Shun Ding, Fangyu Fu, Huibin Niu, Jiaying Yan, Yanfen Fang and Xiang Liu
{"title":"从生物质废弃物中合成掺杂 N 的多孔碳,用于活化水污染中的过硫酸盐:机理研究与生物毒性评估","authors":"Shun Ding, Fangyu Fu, Huibin Niu, Jiaying Yan, Yanfen Fang and Xiang Liu","doi":"10.1039/D4EN00481G","DOIUrl":null,"url":null,"abstract":"<p >N-doping is a widely used strategy for the synthesis of highly efficient carbon nanocatalysts; however, an in-depth understanding of the effect of nitrogen source on the intrinsic structure and catalytic performance is highly desired. Therefore, to kill two birds with one stone, a series of N-doped carbon nanomaterials were synthesized by the pyrolysis of biomass waste (dealkaline lignin) and various nitrogen sources (including melamine, dicyandiamide, and urea). Even though N-doped nanocatalysts showed better catalytic activity than HCNs (pyrolysis of only dealkaline lignin) for sulfamethoxazole (SMX) degradation <em>via</em> peroxymonosulfate (PMS) activation, NCN-1 and NCN-2 presented contractive and small spherical structures when melamine and dicyandiamide with high nitrogen content were added, showing relatively low catalytic efficiency. NPCN derived from dealkaline lignin and urea led to the formation of a porous cluster structure with abundant active species of graphitic C/N and C–OH, which showed the best catalytic performance for SMX degradation. Significantly, NPCN exhibited excellent universality, adaptability, and reusability. Moreover, the possible mechanism was proposed based on quenching study, electron paramagnetic resonance (EPR) analysis, electronic quenching experiment, density functional theory (DFT) calculation, and high-resolution mass spectrometry (HR-MS), confirming that e, <small><sup>1</sup></small>O<small><sub>2</sub></small>, ·OH, SO<small><sub>4</sub></small>˙<small><sup>−</sup></small>, and O<small><sub>2</sub></small>˙<small><sup>−</sup></small> were the active species, of which <small><sup>1</sup></small>O<small><sub>2</sub></small> was the dominant one in the NPCN/PMS system. In addition, the biotoxicity of SMX was evaluated by ecological structure–activity-relationship model (ECOSAR) analysis and germination tests of wheat seeds. This work provides how the nitrogen source would affect the microstructure-dependent catalytic activity of metal-free carbon nanocatalysts for water decontamination.</p>","PeriodicalId":73,"journal":{"name":"Environmental Science: Nano","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synthesis of N-doped porous carbon derived from biomass waste for activating peroxymonosulfate in water decontamination: mechanism insight and biotoxicity assessment†\",\"authors\":\"Shun Ding, Fangyu Fu, Huibin Niu, Jiaying Yan, Yanfen Fang and Xiang Liu\",\"doi\":\"10.1039/D4EN00481G\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >N-doping is a widely used strategy for the synthesis of highly efficient carbon nanocatalysts; however, an in-depth understanding of the effect of nitrogen source on the intrinsic structure and catalytic performance is highly desired. Therefore, to kill two birds with one stone, a series of N-doped carbon nanomaterials were synthesized by the pyrolysis of biomass waste (dealkaline lignin) and various nitrogen sources (including melamine, dicyandiamide, and urea). Even though N-doped nanocatalysts showed better catalytic activity than HCNs (pyrolysis of only dealkaline lignin) for sulfamethoxazole (SMX) degradation <em>via</em> peroxymonosulfate (PMS) activation, NCN-1 and NCN-2 presented contractive and small spherical structures when melamine and dicyandiamide with high nitrogen content were added, showing relatively low catalytic efficiency. NPCN derived from dealkaline lignin and urea led to the formation of a porous cluster structure with abundant active species of graphitic C/N and C–OH, which showed the best catalytic performance for SMX degradation. Significantly, NPCN exhibited excellent universality, adaptability, and reusability. Moreover, the possible mechanism was proposed based on quenching study, electron paramagnetic resonance (EPR) analysis, electronic quenching experiment, density functional theory (DFT) calculation, and high-resolution mass spectrometry (HR-MS), confirming that e, <small><sup>1</sup></small>O<small><sub>2</sub></small>, ·OH, SO<small><sub>4</sub></small>˙<small><sup>−</sup></small>, and O<small><sub>2</sub></small>˙<small><sup>−</sup></small> were the active species, of which <small><sup>1</sup></small>O<small><sub>2</sub></small> was the dominant one in the NPCN/PMS system. In addition, the biotoxicity of SMX was evaluated by ecological structure–activity-relationship model (ECOSAR) analysis and germination tests of wheat seeds. This work provides how the nitrogen source would affect the microstructure-dependent catalytic activity of metal-free carbon nanocatalysts for water decontamination.</p>\",\"PeriodicalId\":73,\"journal\":{\"name\":\"Environmental Science: Nano\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-07-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Science: Nano\",\"FirstCategoryId\":\"6\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/en/d4en00481g\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Science: Nano","FirstCategoryId":"6","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/en/d4en00481g","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Synthesis of N-doped porous carbon derived from biomass waste for activating peroxymonosulfate in water decontamination: mechanism insight and biotoxicity assessment†
N-doping is a widely used strategy for the synthesis of highly efficient carbon nanocatalysts; however, an in-depth understanding of the effect of nitrogen source on the intrinsic structure and catalytic performance is highly desired. Therefore, to kill two birds with one stone, a series of N-doped carbon nanomaterials were synthesized by the pyrolysis of biomass waste (dealkaline lignin) and various nitrogen sources (including melamine, dicyandiamide, and urea). Even though N-doped nanocatalysts showed better catalytic activity than HCNs (pyrolysis of only dealkaline lignin) for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation, NCN-1 and NCN-2 presented contractive and small spherical structures when melamine and dicyandiamide with high nitrogen content were added, showing relatively low catalytic efficiency. NPCN derived from dealkaline lignin and urea led to the formation of a porous cluster structure with abundant active species of graphitic C/N and C–OH, which showed the best catalytic performance for SMX degradation. Significantly, NPCN exhibited excellent universality, adaptability, and reusability. Moreover, the possible mechanism was proposed based on quenching study, electron paramagnetic resonance (EPR) analysis, electronic quenching experiment, density functional theory (DFT) calculation, and high-resolution mass spectrometry (HR-MS), confirming that e, 1O2, ·OH, SO4˙−, and O2˙− were the active species, of which 1O2 was the dominant one in the NPCN/PMS system. In addition, the biotoxicity of SMX was evaluated by ecological structure–activity-relationship model (ECOSAR) analysis and germination tests of wheat seeds. This work provides how the nitrogen source would affect the microstructure-dependent catalytic activity of metal-free carbon nanocatalysts for water decontamination.
期刊介绍:
Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas:
Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability
Nanomaterial interactions with biological systems and nanotoxicology
Environmental fate, reactivity, and transformations of nanoscale materials
Nanoscale processes in the environment
Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis